US20210101111A1 - Process for the removal of sulphur oxides and nitrogen oxides contained in off-gas from an industrial plant - Google Patents
Process for the removal of sulphur oxides and nitrogen oxides contained in off-gas from an industrial plant Download PDFInfo
- Publication number
- US20210101111A1 US20210101111A1 US16/479,651 US201816479651A US2021101111A1 US 20210101111 A1 US20210101111 A1 US 20210101111A1 US 201816479651 A US201816479651 A US 201816479651A US 2021101111 A1 US2021101111 A1 US 2021101111A1
- Authority
- US
- United States
- Prior art keywords
- gas
- filter bag
- oxides
- sulphur
- scr
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Abandoned
Links
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 title claims abstract description 51
- 239000007789 gas Substances 0.000 title claims abstract description 39
- 238000000034 method Methods 0.000 title claims abstract description 32
- XTQHKBHJIVJGKJ-UHFFFAOYSA-N sulfur monoxide Chemical class S=O XTQHKBHJIVJGKJ-UHFFFAOYSA-N 0.000 title claims abstract description 20
- 230000000712 assembly Effects 0.000 claims abstract description 14
- 238000000429 assembly Methods 0.000 claims abstract description 14
- 239000004744 fabric Substances 0.000 claims abstract description 14
- 238000001914 filtration Methods 0.000 claims abstract description 5
- 239000003054 catalyst Substances 0.000 claims description 37
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 33
- BIGPRXCJEDHCLP-UHFFFAOYSA-N ammonium bisulfate Chemical compound [NH4+].OS([O-])(=O)=O BIGPRXCJEDHCLP-UHFFFAOYSA-N 0.000 claims description 17
- 229910021529 ammonia Inorganic materials 0.000 claims description 13
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 10
- 239000003463 adsorbent Substances 0.000 claims description 9
- 239000000203 mixture Substances 0.000 claims description 9
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 8
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 7
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 6
- 238000006243 chemical reaction Methods 0.000 claims description 6
- 239000000428 dust Substances 0.000 claims description 6
- 238000004519 manufacturing process Methods 0.000 claims description 6
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 6
- 229910052802 copper Inorganic materials 0.000 claims description 5
- 239000010949 copper Substances 0.000 claims description 5
- 229910052742 iron Inorganic materials 0.000 claims description 5
- UIIMBOGNXHQVGW-UHFFFAOYSA-M Sodium bicarbonate Chemical compound [Na+].OC([O-])=O UIIMBOGNXHQVGW-UHFFFAOYSA-M 0.000 claims description 4
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims description 4
- 238000010531 catalytic reduction reaction Methods 0.000 claims description 4
- 239000003638 chemical reducing agent Substances 0.000 claims description 4
- 239000000571 coke Substances 0.000 claims description 4
- 238000001816 cooling Methods 0.000 claims description 4
- 229910052593 corundum Inorganic materials 0.000 claims description 4
- 239000006185 dispersion Substances 0.000 claims description 4
- GNTDGMZSJNCJKK-UHFFFAOYSA-N divanadium pentaoxide Chemical compound O=[V](=O)O[V](=O)=O GNTDGMZSJNCJKK-UHFFFAOYSA-N 0.000 claims description 4
- 239000011572 manganese Substances 0.000 claims description 4
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 3
- 239000005864 Sulphur Substances 0.000 claims description 3
- 230000003647 oxidation Effects 0.000 claims description 3
- 238000007254 oxidation reaction Methods 0.000 claims description 3
- 229910052763 palladium Inorganic materials 0.000 claims description 3
- 229910052697 platinum Inorganic materials 0.000 claims description 3
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims description 3
- 239000010937 tungsten Substances 0.000 claims description 3
- 239000010457 zeolite Substances 0.000 claims description 3
- 229910052684 Cerium Inorganic materials 0.000 claims description 2
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 2
- 229910021536 Zeolite Inorganic materials 0.000 claims description 2
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 2
- 230000002378 acidificating effect Effects 0.000 claims description 2
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 2
- 239000000446 fuel Substances 0.000 claims description 2
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 2
- 239000000463 material Substances 0.000 claims description 2
- 150000002736 metal compounds Chemical class 0.000 claims description 2
- 229910052750 molybdenum Inorganic materials 0.000 claims description 2
- 239000011733 molybdenum Substances 0.000 claims description 2
- 230000001172 regenerating effect Effects 0.000 claims description 2
- 229910000030 sodium bicarbonate Inorganic materials 0.000 claims description 2
- 235000017557 sodium bicarbonate Nutrition 0.000 claims description 2
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 2
- 229910052721 tungsten Inorganic materials 0.000 claims description 2
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims 1
- 238000004140 cleaning Methods 0.000 abstract description 5
- 239000013618 particulate matter Substances 0.000 abstract description 5
- 238000001179 sorption measurement Methods 0.000 abstract description 3
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 3
- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 description 3
- 229910052921 ammonium sulfate Inorganic materials 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 239000011148 porous material Substances 0.000 description 3
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- 235000011130 ammonium sulphate Nutrition 0.000 description 2
- 239000001166 ammonium sulphate Substances 0.000 description 2
- 238000003763 carbonization Methods 0.000 description 2
- 239000003245 coal Substances 0.000 description 2
- 239000003546 flue gas Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 239000002243 precursor Substances 0.000 description 2
- 238000006722 reduction reaction Methods 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 239000012855 volatile organic compound Substances 0.000 description 2
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 1
- 230000010718 Oxidation Activity Effects 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 1
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical class [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 239000004202 carbamide Substances 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- ZMIGMASIKSOYAM-UHFFFAOYSA-N cerium Chemical compound [Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce] ZMIGMASIKSOYAM-UHFFFAOYSA-N 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 230000009849 deactivation Effects 0.000 description 1
- 230000009977 dual effect Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 125000004435 hydrogen atom Chemical class [H]* 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 239000003949 liquefied natural gas Substances 0.000 description 1
- 229910000476 molybdenum oxide Inorganic materials 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical class [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 230000000737 periodic effect Effects 0.000 description 1
- 239000002574 poison Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910001930 tungsten oxide Inorganic materials 0.000 description 1
- 238000011144 upstream manufacturing Methods 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/81—Solid phase processes
- B01D53/83—Solid phase processes with moving reactants
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D46/00—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours
- B01D46/0027—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours with additional separating or treating functions
-
- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D46/0027—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours with additional separating or treating functions
- B01D46/0036—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours with additional separating or treating functions by adsorption or absorption
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01D46/02—Particle separators, e.g. dust precipitators, having hollow filters made of flexible material
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D46/00—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours
- B01D46/56—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours with multiple filtering elements, characterised by their mutual disposition
- B01D46/62—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours with multiple filtering elements, characterised by their mutual disposition connected in series
- B01D46/64—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours with multiple filtering elements, characterised by their mutual disposition connected in series arranged concentrically or coaxially
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/48—Sulfur compounds
- B01D53/50—Sulfur oxides
- B01D53/508—Sulfur oxides by treating the gases with solids
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/60—Simultaneously removing sulfur oxides and nitrogen oxides
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
- B01D53/8631—Processes characterised by a specific device
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2239/00—Aspects relating to filtering material for liquid or gaseous fluids
- B01D2239/04—Additives and treatments of the filtering material
- B01D2239/0471—Surface coating material
- B01D2239/0478—Surface coating material on a layer of the filter
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/20—Reductants
- B01D2251/206—Ammonium compounds
- B01D2251/2062—Ammonia
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01D2251/00—Reactants
- B01D2251/30—Alkali metal compounds
- B01D2251/304—Alkali metal compounds of sodium
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D2251/60—Inorganic bases or salts
- B01D2251/606—Carbonates
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D—SEPARATION
- B01D2253/00—Adsorbents used in seperation treatment of gases and vapours
- B01D2253/10—Inorganic adsorbents
- B01D2253/112—Metals or metal compounds not provided for in B01D2253/104 or B01D2253/106
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D2255/102—Platinum group metals
- B01D2255/1021—Platinum
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- B01D2255/102—Platinum group metals
- B01D2255/1023—Palladium
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- B01D2255/20707—Titanium
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D2255/90—Physical characteristics of catalysts
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01D2257/502—Carbon monoxide
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/708—Volatile organic compounds V.O.C.'s
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
Definitions
- Selective catalytic reduction is primarily a means of converting nitrogen oxides (NOx) into N 2 and H 2 O.
- a reductant typically anhydrous ammonia or aqueous ammonia, is added to a stream of flue gas or exhaust gas and then adsorbed onto a catalyst.
- ABS ammonium bisulphate
- SCR catalysts composed of vanadium oxides supported on titania are well known and typically used in stationary applications. Those catalysts are optionally promoted with tungsten and/or molybdenum oxides or various precious metals (such as palladium and platinum). The SCR catalysts are most often employed coated on a monolithic substrate. Other known SCR catalysts include zeolites promoted with copper and/or iron.
- the NOx reduction reaction takes place as the gas contacts the SCR catalyst.
- Ammonia, or a precursor, such as urea is injected and mixed with the gas upstream the SCR catalyst.
- Coke oven gas is a valuable by-product of coal carbonization.
- COG is a potential feedstock for hydrogen separation, methane enrichment, methanol production and synthesis gas production through partial oxidation of COG. It can also be effectively utilized to produce electricity and liquefied natural gas.
- the typical SOx level in COG is 150 mg/Nm 3 -180 mg/Nm 3 .
- Certain SCR catalysts such as the vanadium-based catalysts, are particularly sensitive to contamination from ammonium sulphate and especially ammonium bisulphate, which is condensed in the pore structure of the catalyst at lower temperatures, thereby physically blocking the pores and deactivating the catalyst.
- One way to avoid the off-gas cleaning below the dew point of ammonium bisulphate is to perform the SCR and SOx adsorption prior to cooling the gas.
- the idea underlying the present invention is to operate a catalysed bag filter in NH3-SCR below the dew point of ammonium bisulphate and simultaneously remove sulphur oxides and the formed ammonium bisulphate by means of a pulverous sulphur adsorbent.
- this invention provides a process for the removal of dust, sulphur oxides, and nitrogen oxides contained in off-gas from an industrial plant comprising the steps of cooling the off-gas to a temperature of between 240 and 160° C.;
- the filter bag house adding a pulverous sulphur oxide adsorbent and an amount of nitrogen oxide reducing agent in form of ammonia or a precursor thereof to the cooled off-gas and adsorbing on the pulverous sulphur oxide adsorbent the sulphur oxides and ammonium bisulphate formed by reaction with a part of the added amount of ammonia;
- the off-gas is cooled by means of indirect heat-exchange in a heat exchanger, which typically is present in most of the existing cleaning systems for the removal of sulphur compounds and ammonium bisulphate.
- a heat exchanger typically is present in most of the existing cleaning systems for the removal of sulphur compounds and ammonium bisulphate.
- a sodium bicarbonate powder comprising adsorbent into the filter bag house together with ammonia as NOx reduction agent.
- Ammonium bisulphate and sulphur oxides will thereby be adsorbed on the adsorbent powder and are filtered off together with dust and particulate matter on dispersion side of the filter bags assemblies.
- the filter bag house will contain a plurality of fabric filter bags assemblies arranged in usual manner in the house.
- the filter bag assemblies may each consist of a single fabric filter bag with an SCR catalyst coated on fabric in the permeation side of the bag.
- the filter bag assemblies each comprises an outer filter bag and one or more inner filter bags separately and concentrically arranged within the outer tubular filter bag.
- outer filter bag refers to the filter bag through which the process gas passes first
- inner filter bag refers to the filter bag(s) through which the process gas passes successively after having passed through the outer bag.
- the later embodiment has the advantage that either different types and/or amounts of catalysts can be coated on different filter bags in each filter bag assembly.
- the SCR catalyst applied on the filter bags comprises vanadium pentoxide and titanium oxide and optionally additionally oxides of tungsten and/or molybdenum.
- the catalytically active material can further comprise palladium or platinum in metallic and/or oxidic form.
- These catalysts are active both in the removal of VOCs and carbon monoxide and in the removal of nitrogen oxides (NOx) by the SCR reaction with NH 3 .
- the Pd/V/Ti catalyst is a preferred catalyst because (i) it has a dual functionality (removal of NOx and removal of VOCs), (ii) it is sulphur-tolerant, and (iii) it has a lower SO 2 oxidation activity compared to other catalyst compositions.
- the SCR catalyst comprises a mixture of oxides of manganese, cerium and iron supported on titania.
- Such an SCR catalyst has a sufficient catalytic activity at temperatures well below 190° C., e.g. 130° C. Thereby, it is possible to remove or sufficiently reduce ammonia slip from the SCR catalyst at lower temperatures.
- Sulphur oxide adsorbent particles present in the process gas will be deposited on the outer surface, i.e. the dispersion side of the fabric filter bag facing the uncleaned off-gas.
- the process according to the invention is well suited for the removal of sulphur oxides and ammonium bisulphate in off-gas from coke production and from regenerative oxidation processes with a sulphur containing fuel.
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Abstract
Process for cleaning an off-gas containing sulphur oxides (SOx), nitrogen oxides (NOx) and particulate matter employing SOx adsorption and ammonia-SCR in one filtration unit, in particular a filter bag house with one or more catalysed fabric filter assemblies.
Description
- The present invention relates to a process for cleaning an off-gas containing sulphur oxides (SOx), nitrogen oxides (NOx) and particulate matter employing SOx adsorption and ammonia-SCR in one filtration unit, in particular a filter bag house with one or more catalysed fabric filter assemblies.
- Selective catalytic reduction (SCR)is primarily a means of converting nitrogen oxides (NOx) into N2 and H2O. A reductant, typically anhydrous ammonia or aqueous ammonia, is added to a stream of flue gas or exhaust gas and then adsorbed onto a catalyst.
- It is a well-known problem that SCR employing ammonia as reductant flue gases at low temperatures leads to formation of ammonium bisulphate (ABS) resulting in deactivation of the SCR catalyst and sticky layers of ABS on downstream equipment.
- SCR catalysts composed of vanadium oxides supported on titania are well known and typically used in stationary applications. Those catalysts are optionally promoted with tungsten and/or molybdenum oxides or various precious metals (such as palladium and platinum). The SCR catalysts are most often employed coated on a monolithic substrate. Other known SCR catalysts include zeolites promoted with copper and/or iron.
- The NOx reduction reaction takes place as the gas contacts the SCR catalyst. Ammonia, or a precursor, such as urea is injected and mixed with the gas upstream the SCR catalyst.
- The chemical equation for a stoichiometric reaction using either anhydrous or aqueous ammonia for a selective catalytic reduction process is as shown below:
-
4NO+4NH3+O2→4N2+6H2O -
2NO2+4NH3+O2→3N2+6H2O -
NO+NO2+2NH3→2N2+3H2O - Off-gases from certain industrial processes contain beside NOx also SOx.
- An example of such processes is coal carbonization to produce coke for the steel industry. Coke oven gas (COG) is a valuable by-product of coal carbonization. COG is a potential feedstock for hydrogen separation, methane enrichment, methanol production and synthesis gas production through partial oxidation of COG. It can also be effectively utilized to produce electricity and liquefied natural gas.
- The typical SOx level in COG is 150 mg/Nm3-180 mg/Nm3.
- In order to be suitable as a valuable off-gas, COG and other SOx and NOx containing off-gases must be cleaned by removal of these impurities optionally together with dust or particulate matter further contained in the off-gas.
- As already mentioned above, a problem in the ammonia-SCR denitrification process of gases with a high content of SOX is formation of ammonium bisulphate. SO3 reacts with ammonia to produce ammonium sulphate ((NH4) 2SO4) and ABS(NH4HSO4) by the following reaction scheme:
-
2SO2+O2→2SO3 -
2NH3+SO3+H2O2O→(NH4)2SO4 -
NH3+SO3+H2O→NH4HSO4 - The bulk dew point of ABS at the SCR reactor inlet is typically around 290° C., but the observed dew point is higher due to capillary forces in the micropore structure of the SCR catalyst.
- Certain SCR catalysts, such as the vanadium-based catalysts, are particularly sensitive to contamination from ammonium sulphate and especially ammonium bisulphate, which is condensed in the pore structure of the catalyst at lower temperatures, thereby physically blocking the pores and deactivating the catalyst.
- One way to avoid the off-gas cleaning below the dew point of ammonium bisulphate is to perform the SCR and SOx adsorption prior to cooling the gas.
- On the other hand, operation of the SCR at a low temperature below the dew point of ammonium bisulphate is desirable because of a reduced energy demand and the possibility of separation of valuable organic compounds like benzene, toluene and xylene contained in certain off-gases, when cooling the hot off-gas from production plant prior to the SCR reaction.
- Another way to handle this problem is to periodically operating the SCR at a high temperature, where the ammonium bisulphate is released from the catalyst and the catalyst pores are made available for the catalytic reaction. In this way, the catalyst is reactivated.
- When employing catalysed fabric bag filters in SCR service and particulate matter filtration, the process must be performed at operation temperatures below the destruction temperature of the bags. Generally, filter bags are only durable up to around 240° C., which makes periodic heat treatment at higher temperatures impossible.
- The idea underlying the present invention is to operate a catalysed bag filter in NH3-SCR below the dew point of ammonium bisulphate and simultaneously remove sulphur oxides and the formed ammonium bisulphate by means of a pulverous sulphur adsorbent.
- Thus, this invention provides a process for the removal of dust, sulphur oxides, and nitrogen oxides contained in off-gas from an industrial plant comprising the steps of cooling the off-gas to a temperature of between 240 and 160° C.;
- passing the cooled off-gas to a filter bag house;
- in the filter bag house adding a pulverous sulphur oxide adsorbent and an amount of nitrogen oxide reducing agent in form of ammonia or a precursor thereof to the cooled off-gas and adsorbing on the pulverous sulphur oxide adsorbent the sulphur oxides and ammonium bisulphate formed by reaction with a part of the added amount of ammonia;
- passing the thus treated off-gas together with the remaining amount of the ammonia through one or more fabric filter assemblies arranged in the filter bag house and filtering off the dust, the adsorbed sulphur oxides and the adsorbed ammonium bisulphate on dispersion side of the one or more fabric filter bag assemblies; and
- reducing or removing content of the nitrogen oxides in the filtered off-gas by selective catalytic reduction with ammonia by contact with an SCR catalyst coated on fabric within permeation side of the one or more filter bag assemblies.
- Preferably, the off-gas is cooled by means of indirect heat-exchange in a heat exchanger, which typically is present in most of the existing cleaning systems for the removal of sulphur compounds and ammonium bisulphate. This makes the process according to the invention attractive for retrofit of these cleaning systems.
- When operating the process according to the invention, it is preferred to blow a sodium bicarbonate powder comprising adsorbent into the filter bag house together with ammonia as NOx reduction agent. Ammonium bisulphate and sulphur oxides will thereby be adsorbed on the adsorbent powder and are filtered off together with dust and particulate matter on dispersion side of the filter bags assemblies.
- Typically, the filter bag house will contain a plurality of fabric filter bags assemblies arranged in usual manner in the house.
- The filter bag assemblies may each consist of a single fabric filter bag with an SCR catalyst coated on fabric in the permeation side of the bag.
- In another embodiment of the invention, the filter bag assemblies each comprises an outer filter bag and one or more inner filter bags separately and concentrically arranged within the outer tubular filter bag.
- The term “outer filter bag” refers to the filter bag through which the process gas passes first, and the term “inner filter bag” refers to the filter bag(s) through which the process gas passes successively after having passed through the outer bag.
- The later embodiment has the advantage that either different types and/or amounts of catalysts can be coated on different filter bags in each filter bag assembly.
- The SCR catalyst applied on the filter bags comprises vanadium pentoxide and titanium oxide and optionally additionally oxides of tungsten and/or molybdenum.
- The catalytically active material can further comprise palladium or platinum in metallic and/or oxidic form.
- These catalysts are active both in the removal of VOCs and carbon monoxide and in the removal of nitrogen oxides (NOx) by the SCR reaction with NH3.
- The Pd/V/Ti catalyst is a preferred catalyst because (i) it has a dual functionality (removal of NOx and removal of VOCs), (ii) it is sulphur-tolerant, and (iii) it has a lower SO2 oxidation activity compared to other catalyst compositions.
- In further a preferred embodiment of the invention the SCR catalyst comprises a mixture of oxides of manganese, cerium and iron supported on titania. Such an SCR catalyst has a sufficient catalytic activity at temperatures well below 190° C., e.g. 130° C. Thereby, it is possible to remove or sufficiently reduce ammonia slip from the SCR catalyst at lower temperatures.
- Sulphur oxide adsorbent particles present in the process gas will be deposited on the outer surface, i.e. the dispersion side of the fabric filter bag facing the uncleaned off-gas.
- Thus, the catalysts loaded onto the outer bag and/or the inner bag(s) are effectively protected against potential catalyst poisons in particular sulphur oxides present contained in the off-gas.
- This makes it possible to employ zeolitic material promoted with iron and/or copper as effective SCR catalysts, especially in the low temperature range of the process, including e.g. Cu-SAPO-34 and Cu-SSZ-13.
- Further SCR composition useful in the process according to the invention include compositions comprising one or more acidic zeolite or zeotype components selected from the group consisting of BEA, MFI, FAU, FER, CHA, MOR or mixtures thereof physically admixed with one or more redox active metal compounds selected from the group consisting of Cu/AI2O3, Mn/Al2O3, CeO2—ZrO2, Ce—Mn/Al2O3 and mixtures thereof, as described in U.S. Pat. No. 9,168,517.
- As already mentioned above, the process according to the invention is well suited for the removal of sulphur oxides and ammonium bisulphate in off-gas from coke production and from regenerative oxidation processes with a sulphur containing fuel.
Claims (14)
1. Process for the removal of dust, sulphur oxides and nitrogen oxides contained in off-gas from an industrial plant comprising the steps of
cooling the off-gas to a temperature of between 240 and 160° C.;
passing the cooled off-gas to a filter bag house;
in the filter bag house adding a pulverous sulphur oxide adsorbent and an amount of nitrogen oxide reducing agent in form of ammonia to the cooled off-gas and adsorbing on the pulverous sulphur oxide adsorbent the sulphur oxides and ammonium bisulphate formed by reaction with a part of the added amount of ammonia;
passing the thus treated off-gas together with the remaining amount of the ammonia through one or more fabric filter bag assemblies arranged in the filter bag house and filtering off the dust, the adsorbed sulphur oxides and the adsorbed ammonium bisulphate on dispersion side of the one or more fabric filter bag assemblies; and
reducing or removing content of the nitrogen oxides in the filtered off-gas by selective catalytic reduction with ammonia by contact with an SCR catalyst coated on fabric within permeation side of the one or more filter bag assemblies.
2. The process of claim 1 , wherein main part of the adsorbed sulphur oxides consists of SO3.
3. The process of claim 1 , wherein the off-gas is cooled by heat exchange.
4. The process of claim 1 , wherein the pulverous sulphur oxide adsorbent comprises sodium bicarbonate.
5. The process of claim 1 , wherein each of the one or more filter bag assemblies consists of a single fabric filter bag.
6. The process of claim 1 , wherein the one or more filter bag assemblies each comprises an outer filter bag and one or more inner filter bags separately and concentrically arranged within the outer filter bag.
7. The process of claims 1 , wherein the SCR active catalyst comprises vanadium pentoxide and titanium oxide.
8. The process of claim 7 , wherein the SCR active catalyst further comprises oxides of tungsten and/or molybdenum.
9. The process of claim 7 , wherein the SCR active catalyst further comprises palladium or platinum in metallic and/or oxidic form.
10. The process of claim 1 , wherein the SCR active catalyst comprises a mixture of oxides of manganese, iron and cerium supported on titania.
11. The process of claim 1 , wherein the SCR active catalyst comprises zeolitic material promoted with iron and/or copper.
12. The process of claim 1 , wherein the SCR active catalyst comprises one or more acidic zeolite or zeotype components selected from the group consisting of BEA, MFI, FAU, FER, CHA, MOR or mixtures thereof physically admixed with one or more redox active metal compounds selected from the group consisting of Cu/AI2O3, Mn/Al2O3, CeO2—ZrO2, Ce—Mn/Al2O3 and mixtures thereof.
13. The process of claim 1 , wherein the off-gas originates from a regenerative oxidation process with a sulphur containing fuel.
14. The process of claim 1 , wherein the off-gas originates from production of coke.
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PCT/EP2018/054646 WO2018158183A1 (en) | 2017-03-02 | 2018-02-26 | Process for the removal of sulphur oxides and nitrogen oxides contained in off-gas from an industrial plant |
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US (1) | US20210101111A1 (en) |
EP (1) | EP3589387A1 (en) |
JP (1) | JP2020510524A (en) |
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CN115582016A (en) * | 2022-11-08 | 2023-01-10 | 山东万达环保科技有限公司 | Special ultralow-temperature desulfurization and denitrification process for lime kiln |
WO2023186965A1 (en) * | 2022-04-01 | 2023-10-05 | Topsoe A/S | A process for catalytic filtration of sulfur-containing gases using selective catalytic reduction |
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CA3183030A1 (en) * | 2020-07-15 | 2022-01-20 | Monaca A. Mcnall | Methods for regenerating a filter medium and cleaning flue gas |
JP2024501854A (en) * | 2020-12-30 | 2024-01-16 | ダブリュ.エル.ゴア アンド アソシエイツ,インコーポレイティド | Improving the catalytic efficiency of flue gas filtration through salt formation by using at least one oxidizing agent |
CN113713825B (en) * | 2021-08-31 | 2022-05-27 | 华电青岛环保技术有限公司 | Sulfur-resistant and water-resistant wide-temperature decarburization catalyst and preparation method and application thereof |
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JPS5325601A (en) * | 1976-08-23 | 1978-03-09 | Nippon Steel Corp | Treatment of exhaust combustion gases from coke ovens |
US4220633A (en) * | 1979-04-30 | 1980-09-02 | The Babcock & Wilcox Company | Filter house and method for simultaneously removing NOx and particulate matter from a gas stream |
US4793981A (en) * | 1986-11-19 | 1988-12-27 | The Babcock & Wilcox Company | Integrated injection and bag filter house system for SOx -NOx -particulate control with reagent/catalyst regeneration |
US5585081A (en) * | 1988-07-25 | 1996-12-17 | The Babcock & Wilcox Company | SOx, NOx and particulate removal system |
JP3491141B2 (en) * | 1999-03-16 | 2004-01-26 | Jfeエンジニアリング株式会社 | Exhaust gas treatment method and apparatus |
US7481983B2 (en) * | 2004-08-23 | 2009-01-27 | Basf Catalysts Llc | Zone coated catalyst to simultaneously reduce NOx and unreacted ammonia |
WO2006103040A1 (en) * | 2005-04-01 | 2006-10-05 | Haldor Topsøe A/S | Process for catalytic reduction of nox by ammonia in presence of so3 in the gas |
CN101028594A (en) * | 2006-03-01 | 2007-09-05 | 中国科学院生态环境研究中心 | Composite oxide catalyst for cryogenic selective catalystic reductic oxide nitrogen |
EP2112341B1 (en) * | 2008-04-22 | 2018-07-11 | Umicore AG & Co. KG | Method for purification of an exhaust gas from a diesel engine |
US7968492B2 (en) * | 2009-05-11 | 2011-06-28 | Millennium Inorganic Chemicals, Inc. | Layered catalyst to improve selectivity or activity of manganese containing vanadium-free mobile catalyst |
JP2011062663A (en) * | 2009-09-18 | 2011-03-31 | Mitsubishi Heavy Industries Environmental & Chemical Engineering Co Ltd | Method for treating exhaust gas |
WO2013060341A1 (en) * | 2011-10-24 | 2013-05-02 | Haldor Topsøe A/S | Catalyst composition for use in selective catalytic reduction of nitrogen oxides |
AR100119A1 (en) * | 2014-03-21 | 2016-09-14 | Haldor Topsoe As | MOUNTING FILTER BAGS |
CN104190193B (en) * | 2014-08-22 | 2015-11-18 | 合肥工业大学 | A kind of method of sack cleaner inter-sync desulfur denitrate dust collecting |
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2018
- 2018-02-02 TW TW107103825A patent/TW201838708A/en unknown
- 2018-02-26 CN CN201880012301.2A patent/CN110312563A/en active Pending
- 2018-02-26 KR KR1020197023499A patent/KR20190121301A/en not_active Application Discontinuation
- 2018-02-26 US US16/479,651 patent/US20210101111A1/en not_active Abandoned
- 2018-02-26 EP EP18707705.2A patent/EP3589387A1/en not_active Withdrawn
- 2018-02-26 JP JP2019547376A patent/JP2020510524A/en active Pending
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WO2023186965A1 (en) * | 2022-04-01 | 2023-10-05 | Topsoe A/S | A process for catalytic filtration of sulfur-containing gases using selective catalytic reduction |
CN115582016A (en) * | 2022-11-08 | 2023-01-10 | 山东万达环保科技有限公司 | Special ultralow-temperature desulfurization and denitrification process for lime kiln |
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CN110312563A (en) | 2019-10-08 |
KR20190121301A (en) | 2019-10-25 |
TW201838708A (en) | 2018-11-01 |
JP2020510524A (en) | 2020-04-09 |
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